Engineering Dual Single‐Atom Sites on 2D Ultrathin N‐doped Carbon Nanosheets Attaining Ultra‐Low‐Temperature Zinc‐Air Battery

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(12)

Published: Jan. 7, 2022

Herein, a novel dual single-atom catalyst comprising adjacent Fe-N4 and Mn-N4 sites on 2D ultrathin N-doped carbon nanosheets with porous structure (FeMn-DSAC) was constructed as the cathode for flexible low-temperature Zn-air battery (ZAB). FeMn-DSAC exhibits remarkable bifunctional activities oxygen reduction reaction (ORR) evolution (OER). Control experiments density functional theory calculations reveal that catalytic activity arises from cooperative effect of Fe/Mn dual-sites aiding *OOH dissociation well nanosheet promoting active sits exposure mass transfer during process. The excellent enables ZAB to operate efficiently at ultra-low temperature -40 °C, delivering 30 mW cm-2 peak power retaining up 86 % specific capacity room counterpart.

Language: Английский

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Understanding the structure-performance relationship of active sites at atomic scale

Nano Research, Journal Year: 2022, Volume and Issue: 15(8), P. 6888 - 6923

Published: June 14, 2022

Language: Английский

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Constructing Cd0.5Zn0.5S/Bi2WO6 S-scheme heterojunction for boosted photocatalytic antibiotic oxidation and Cr(VI) reduction

Advanced Powder Materials, Journal Year: 2022, Volume and Issue: 2(1), P. 100073 - 100073

Published: June 30, 2022

The development of distinguished photocatalysts with high photo-carrier disassociation and photo-redox power for efficient elimination pollutants in water is great significance but still a grand challenge. Herein, novel Cd0.5Zn0.5S/Bi2WO6 S-scheme heterojunction was built up by integrating Cd0.5Zn0.5S nanoparticles on Bi2WO6 microspheres via simple route. charge transfer mode substantially boosts the high-energetic electrons/holes spatial detachment conservation (reduction) (oxidation), respectively, as well effectively suppresses photo-corrosion Cd0.5Zn0.5S, rendering superior redox ability. optimal achieves exceptional visible-light-driven photocatalytic tetracycline degradation Cr(VI) reduction efficiency, 3.2 (1.9)-time 33.6 (1.6)-time stronger than that neat (Cd0.5Zn0.5S), while retaining stability reusability. Quenching test, mass spectrometry analysis, toxicity assessment based Quantitative Structure Activity Relationships. calculation unravel prime active substances, intermediates, photo-degradation pathway, intermediate eco-toxicity process. This research not only offers potential photocatalyst aquatic environment protection also promotes exploration powerful chalcogenides-based protection.

Language: Английский

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Ta3N5/CdS Core–Shell S-scheme Heterojunction Nanofibers for Efficient Photocatalytic Removal of Antibiotic Tetracycline and Cr(VI): Performance and Mechanism Insights

Advanced Fiber Materials, Journal Year: 2023, Volume and Issue: 5(3), P. 994 - 1007

Published: Feb. 16, 2023

Language: Английский

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Regulations of active moiety in single atom catalysts for electrochemical hydrogen evolution reaction

Nano Research, Journal Year: 2022, Volume and Issue: 15(7), P. 5792 - 5815

Published: May 4, 2022

Language: Английский

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Surface carbon layer controllable Ni3Fe particles confined in hierarchical N-doped carbon framework boosting oxygen evolution reaction

Advanced Powder Materials, Journal Year: 2021, Volume and Issue: 1(2), P. 100020 - 100020

Published: Dec. 10, 2021

Developing high-efficiency and low-cost catalysts towards oxygen evolution reaction (OER) is extremely important for overall water splitting rechargeable metal−air batteries. Herein we propose a promising organometallic coordination polymer (OCP) induced strategy to construct hierarchical N-doped carbon framework with NiFe nanoparticles encapsulated inside (Nx[email protected]–C) as highly active stable OER catalyst. The synthesis of OCP precursor depends on the unique molecular structure iminodiacetonitrile (IDAN), which can coordinate metal ions form Ni2Fe(CN)6 prussian blue analogs (PBA) structure. Unlike previous PBA-induced methods, thickness layer covering surface core be well controlled during pyrolysis through adjusting amount IDAN, builds wonderful bridge investigating relationship between catalytic performance. Both experimental characterizations theoretical studies validate that suitable layers leads optimal activity stability. By optimizing composition, optimized Ni3[email protected]–C exhibits low overpotentials (260 ​mV at 10 ​mA ​cm−2; 320 50 ​cm−2), improved kinetics (79 dec−1), robust long-term stability, exceeds those benchmark RuO2.

Language: Английский

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Emerging low-nuclearity supported metal catalysts with atomic level precision for efficient heterogeneous catalysis

Nano Research, Journal Year: 2022, Volume and Issue: 15(9), P. 7806 - 7839

Published: June 2, 2022

Language: Английский

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Single‐Atom Fe Catalysts for Fenton‐Like Reactions: Roles of Different N Species

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(17)

Published: March 8, 2022

Recognizing and controlling the structure-activity relationships of single-atom catalysts (SACs) is vital for manipulating their catalytic properties various practical applications. Herein, Fe SACs supported on nitrogen-doped carbon (SA-Fe/CN) are reported, which show high reactivity (97% degradation bisphenol A in only 5 min), stability (80% maintained after five runs), wide pH suitability (working range 3-11) toward Fenton-like reactions. The roles different N species these reactions further explored, both experimentally theoretically. It discovered that graphitic an adsorptive site target molecule, pyrrolic coordinates with Fe(III) plays a dominant role reaction, pyridinic N, coordinated Fe(II), minor contributor to SA-Fe/CN. Density functional theory (DFT) calculations reveal lower d-band center location pyrrolic-type sites leads easy generation Fe-oxo intermediates, thus, excellent properties.

Language: Английский

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Quasi-solid-state Zn-air batteries with an atomically dispersed cobalt electrocatalyst and organohydrogel electrolyte

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: June 27, 2022

Abstract Quasi-solid-state Zn-air batteries are usually limited to relatively low-rate ability (<10 mA cm −2 ), which is caused in part by sluggish oxygen electrocatalysis and unstable electrochemical interfaces. Here we present a high-rate robust quasi-solid-state battery enabled atomically dispersed cobalt sites anchored on wrinkled nitrogen doped graphene as the air cathode polyacrylamide organohydrogel electrolyte with its hydrogen-bond network modified addition of dimethyl sulfoxide. This design enables cycling current density 100 over 50 h at 25 °C. A low-temperature stability 300 (at 0.5 ) 90% capacity retention −60 °C broad temperature adaptability (−60 60 °C) also demonstrated.

Language: Английский

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Ru–Co Pair Sites Catalyst Boosts the Energetics for the Oxygen Evolution Reaction

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(32)

Published: May 31, 2022

Abstract Manipulating the coordination environment of active center via anion modulation to reveal tailored activity and selectivity has been widely achieved, especially for carbon‐based single‐atom site catalysts (SACs). However, tuning ligand fields by single‐site metal cation regulation identifying effects on resulting electronic configuration is seldom explored. Herein, we propose a Ru strategy engineer properties constructing Ru/LiCoO 2 SAC with atomically dispersed Ru−Co pair sites. Benefitting from strong coupling between Co sites, catalyst possesses an enhanced electrical conductivity achieves near‐optimal oxygen adsorption energies. Therefore, optimized delivers superior evolution reaction (OER) low overpotential, high mass 1000 A g oxide −1 at small overpotential 335 mV, excellent long‐term stability. It also exhibits rapid kinetics rate capability outstanding durability in zinc–air battery.

Language: Английский

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